![]() ![]() In this review, we overview various types of stepwise 2PA processes from the viewpoints of history, fundamentals, and applications. Because of these advantages, the stepwise 2PA has been widely studied more than a half century ago not only for fundamental physics and chemistry but also for applications to optical memory, holography, and artificial photosynthesis. Moreover, if a photogenerated chemical species is used as an intermediate state of the stepwise 2PA, the power threshold to promote the stepwise 2PA can be greatly reduced compared with that of a simultaneous 2PA, and conventional LEDs and even sunlight could be used to induce the stepwise 2PA. The stepwise 2PA can selectively produce a higher excited state with relatively high spatial selectivity, and therefore, it can be an efficient tool to explore and realize nonlinear photoresponsive materials beyond Kasha’s rule. ![]() Stepwise two-photon absorption (2PA) is one of the nonlinear photoresponses where two photons are sequentially absorbed to proceed a photophysical or photochemical reaction.
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